期刊
INORGANIC CHEMISTRY
卷 60, 期 2, 页码 817-831出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.inorgchem.0c02863
关键词
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资金
- National Natural Science Foundation of China [21703002, 21727805, 21673180]
- Young Talent Fund of University Association for Science and Technology in Shaanxi, China [20200610]
- Special Scientific Research Project of Education Department of Shaanxi Provincial Government [20JK0484]
- Natural Science Basic Research Plan in Shaanxi Province of China [2019JQ180]
- Open Foundation of Key Laboratory of Synthetic and Natural Functional Molecule Chemistry of Ministry of Education [338050067(2018-008)]
- National Undergraduate Training Programs for Innovation and Entrepreneurship [S202010721006]
- Doctoral Scientific Research Starting Foundation of Baoji University of Arts and Science [ZK2017024]
Guided by the self-assembled process and mechanism, the strategy of in situ Schiff base reaction successfully synthesized lanthanide compounds with distinct structures and magnetic properties, including mononuclear and binuclear Dy(III) compounds.
Guided by the self-assembled process and mechanism, the strategy of in situ Schiff base reaction would be capable of bringing a feasible method to construct and synthesize lanthanide compounds with distinct structures and magnetic properties. A mononuclear Dy(III) compound was synthesized through a multidentate Schiff base ligand and a chelating beta-diketonate ligand, which was named as [Dy(L)(bppd)]center dot CH3OH [1; H2L = N,N'-bis(2-hydroxy-5-methyl-3formylbenzyl)-N,N'-bis(pyridin-2-ylmethyl)ethylenediamine and bppd = 3-bis(pyridin-2-yl)propane-1,3-dione]. Furthermore, a new binuclear Dy(III) compound, [Dy2(H2Lox)(bppd)3]center dot 8CH(3)OH [2; H4Lox = N,N'-bis[2-hydroxy-5methyl- 3-(hydroxyiminomethyl) benzyl]- N,N'- bis( pyridin- 2- ylmethyl)ethylenediamine], was obtained via an in situ synthetic process. Under similar synthetic conditions, [Dy(L)(ctbd)] [3; ctbd = 1-(4-chlorophenyl)-4,4,4-trifluoro1,3-butanedione] and [Dy-2(H(2)Lox)(ctbd)(3)]center dot CH3OH center dot C4H10O (4) were synthesized by modifying the beta-diketonate ligand and in situ Schiff base reaction. Compound 3 is a mononuclear configuration, while compound 4 exhibits a binuclear Dy(III) unit. Therein, formylbenzyl groups of H2L in 1 and 3 were changed to (hydroxyiminomethyl)benzyl groups in 2 and 4, respectively. In isomorphous 2 and 4, two Dy(III) centers are connected through two phenol O- atoms of the H(2)Lox(2)(-) ligand to form a binuclear structure. Eight-coordinated Dy(III) ions with different distortions can be observed in 1-4. The crystals of 1 and 3 suffered dissolution/precipitation to obtain 2 and 4, respectively. The relationship between the structure and magnetism in compounds 1-4 was discussed through the combination of structural, experimental, and theoretical investigations. Especially, the rates of quantum tunneling of magnetization of 1-4 were theoretically predicted and are consistent with the experimental results. For 2 and 4, the theoretically calculated dipolar parameters Jdip are consistent with the experimental observation of weak ferromagnetic coupling.
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